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18 pages, 3344 KiB  
Article
Chondroitin Sulfate/Cyanocobalamin–Chitosan Polyelectrolyte Complexes for Improved Oral Delivery of Colistin
by Natallia V. Dubashynskaya, Andrey Y. Borovskoy, Anton N. Bokatyi, Tatiana S. Sall, Tatiana S. Egorova, Elena V. Demyanova, Ekaterina A. Murashko and Yury A. Skorik
Polysaccharides 2025, 6(1), 21; https://doi.org/10.3390/polysaccharides6010021 - 7 Mar 2025
Viewed by 152
Abstract
Introduction. The rise of multidrug resistance in Gram-negative ESKAPE pathogens is a critical challenge for modern healthcare. Colistin (CT), a peptide antibiotic, remains a last-resort treatment for infections caused by these superbugs due to its potent activity against Gram-negative bacteria and the rarity [...] Read more.
Introduction. The rise of multidrug resistance in Gram-negative ESKAPE pathogens is a critical challenge for modern healthcare. Colistin (CT), a peptide antibiotic, remains a last-resort treatment for infections caused by these superbugs due to its potent activity against Gram-negative bacteria and the rarity of resistance. However, its clinical use is severely limited by high nephro- and neurotoxicity, low oral bioavailability, and other adverse effects. A promising strategy to improve the biopharmaceutical properties and safety profile of antibiotics is the development of biopolymer-based delivery systems, also known as nanoantibiotics. Objective. The aim of this study was to develop polyelectrolyte complexes (PECs) for the oral delivery of CT to overcome its major limitations, such as poor bioavailability and toxicity. Methods. PECs were formulated using chondroitin sulfate (CHS) and a cyanocobalamin–chitosan conjugate (CSB12). Vitamin B12 was incorporated as a targeting ligand to enhance intestinal permeability through receptor-mediated transport. The resulting complexes (CHS-CT-CSB12) were characterized for particle size, ζ-potential, encapsulation efficiency, and drug release profile under simulated gastrointestinal conditions (pH 1.6, 6.5, and 7.4). The antimicrobial activity of the encapsulated CT was evaluated in vitro against Pseudomonas aeruginosa. Results. The CHS-CT-CSB12 PECs exhibited a hydrodynamic diameter of 446 nm and a ζ-potential of +28.2 mV. The encapsulation efficiency of CT reached 100% at a drug loading of 200 µg/mg. In vitro release studies showed that approximately 70% of the drug was released within 1 h at pH 1.6 (simulating gastric conditions), while a cumulative CT release of 80% over 6 h was observed at pH 6.5 and 7.4 (simulating intestinal conditions). This release profile suggests the potential use of enteric-coated capsules or specific administration guidelines, such as taking the drug on an empty stomach with plenty of water. The antimicrobial activity of encapsulated CT against P. aeruginosa was comparable to that of the free drug, with a minimum inhibitory concentration of 1 µg/mL for both. The inclusion of vitamin B12 in the PECs significantly improved intestinal permeability, as evidenced by an apparent permeability coefficient (Papp) of 1.1 × 10−6 cm/s for CT. Discussion. The developed PECs offer several advantages over conventional CT formulations. The use of vitamin B12 as a targeting ligand enhances drug absorption across the intestinal barrier, potentially increasing oral bioavailability. In addition, the controlled release of CT in the intestinal environment reduces the risk of systemic toxicity, particularly nephro- and neurotoxicity. These findings highlight the potential of CHS-CT-CSB12 PECs as a nanotechnology-based platform for improving the delivery of CT and other challenging antibiotics. Conclusions. This study demonstrates the promising potential of CHS-CT-CSB12 PECs as an innovative oral delivery system for CT that addresses its major limitations and improves its therapeutic efficacy. Future work will focus on in vivo evaluation of the safety and efficacy of the system, as well as exploring its applicability for delivery of other antibiotics with similar challenges. Full article
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Figure 1
<p>Formation of polyelectrolyte complexes based on chondroitin sulfate, B12-chitosan, and colistin.</p>
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<p>The ζ-potentials (<b>a</b>) and hydrodynamic diameters (<b>b</b>) of CHS-CSB12 PEC at different pH; the ζ-potentials and hydrodynamic diameters of the CHS-CT complexes (<b>c</b>). Data are presented as the mean ± SD, <span class="html-italic">n</span> = 3.</p>
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<p>The ζ-potentials (<b>a</b>) and hydrodynamic diameters (<b>b</b>) of CHS-CSB12 PEC at different pH; the ζ-potentials and hydrodynamic diameters of the CHS-CT complexes (<b>c</b>). Data are presented as the mean ± SD, <span class="html-italic">n</span> = 3.</p>
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<p>SEM images of tri-component polyelectrolyte complexes based on chondroitin sulfate, B12-chitosan, and colistin (CHS-CT-CSB12 PECs) at different magnifications: 1 μm scale, 65,800× magnification (<b>a</b>) and 200 nm scale, 190,000× magnification (<b>b</b>).</p>
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<p>Cumulative release of colistin from the tri-component polyelectrolyte complexes based on chondroitin sulfate, B12-chitosan/chitosan, and colistin (CHS-CT-CSB12 and CHS-CT-CS PECs) in 6 h at 37 °C and different pH. Each point is presented as the mean ± SD, <span class="html-italic">n</span> = 3 (<b>a</b>). Minimum inhibitory concentrations of CHS-CT-CSB12 and CHS-CT-CS PECs and free colistin against <span class="html-italic">P. aeruginosa</span>. Data are presented as the mean ± SD, <span class="html-italic">n</span> = 3 (<b>b</b>). Mucoadhesiveness of the CHS-CT-CSB12 and CHS-CT-CS PECs. Data are presented as the mean ± SD, <span class="html-italic">n</span> = 3 (<b>c</b>).</p>
Full article ">Figure 4 Cont.
<p>Cumulative release of colistin from the tri-component polyelectrolyte complexes based on chondroitin sulfate, B12-chitosan/chitosan, and colistin (CHS-CT-CSB12 and CHS-CT-CS PECs) in 6 h at 37 °C and different pH. Each point is presented as the mean ± SD, <span class="html-italic">n</span> = 3 (<b>a</b>). Minimum inhibitory concentrations of CHS-CT-CSB12 and CHS-CT-CS PECs and free colistin against <span class="html-italic">P. aeruginosa</span>. Data are presented as the mean ± SD, <span class="html-italic">n</span> = 3 (<b>b</b>). Mucoadhesiveness of the CHS-CT-CSB12 and CHS-CT-CS PECs. Data are presented as the mean ± SD, <span class="html-italic">n</span> = 3 (<b>c</b>).</p>
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16 pages, 12999 KiB  
Article
One-Pot Synthesis of Amphiphilic Linear and Hyperbranched Polyelectrolytes and Their Stimuli-Responsive Self-Assembly in Aqueous Solutions
by Angelica Maria Gerardos, Aleksander Forys, Barbara Trzebicka and Stergios Pispas
Polymers 2025, 17(5), 701; https://doi.org/10.3390/polym17050701 - 6 Mar 2025
Viewed by 107
Abstract
Stimuli-responsive polymeric nanostructures are compelling vectors for a wide range of application opportunities. The objective we sought was to broaden the array of self-assembling amphiphilic copolymers with stimuli-responsive characteristics by introducing a hydrophilic tunable monomer, (2-dimethylamino)ethyl methacrylate (DMAEMA), together with a hydrophilic one, [...] Read more.
Stimuli-responsive polymeric nanostructures are compelling vectors for a wide range of application opportunities. The objective we sought was to broaden the array of self-assembling amphiphilic copolymers with stimuli-responsive characteristics by introducing a hydrophilic tunable monomer, (2-dimethylamino)ethyl methacrylate (DMAEMA), together with a hydrophilic one, lauryl methacrylate (LMA), within linear and branched copolymer topologies. Size exclusion chromatography was used to evaluate the resultant linear and hyperbranched copolymers’ molecular weight and dispersity, and FT-IR and 1H-NMR spectroscopy techniques were used to delineate their chemical structure. The structural changes in the obtained self-organized supramolecular structures were thoroughly investigated using aqueous media with varying pH and salinity by dynamic light scattering (DLS), fluorescence spectroscopy (FS), and transmission electron microscopy (TEM). The nanoscale assemblies formed by the amphiphiles indicate significant potential for applications within the field of nanotechnology. Full article
(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)
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<p>Synthesis route of hyperbranched H-P(LMA-co-DMAEMA) copolymer.</p>
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<p>SEC curves of the hyperbranched (<b>a</b>) and linear (<b>b</b>) LMA/DMAEMA copolymers.</p>
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<p><sup>1</sup>H-NMR spectrum of P2 in CDCl<sub>3</sub>. Letters above the spectra peaks correspond to the relevant H nuclei shown in the chemical structure of the copolymer in the inset.</p>
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<p>ATR-FTIR spectra of the hyperbranched copolymers (in the solid state).</p>
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<p>DLS size distributions for P1 (<b>a</b>) and P2 (<b>b</b>) linear copolymer aqueous solutions, C<sub>polymer</sub> = 10<sup>−3</sup> g/mL.</p>
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<p>DLS size distributions for H1 (<b>a</b>) and H2 (<b>b</b>) hyperbranched copolymer aqueous solutions.</p>
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<p>Collective DLS data as a function of salinity. (<b>a</b>) P1 and (<b>b</b>) P2 linear copolymers, C<sub>polymer</sub> = 10<sup>−3</sup> g/mL, pH = 7.</p>
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<p>Collective DLS data as a function of salinity. (<b>a</b>) H1 and (<b>b</b>) H2 hyperbranched copolymers, C<sub>polymer</sub> = 10<sup>−3</sup> g/mL, pH = 7.</p>
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<p>I<sub>1</sub>/I<sub>3</sub> vs. polymer concentration plots for CAC determination regarding (<b>a</b>) P1 and (<b>b</b>) P2 copolymer aqueous solutions, C<sub>pyrene</sub> = 1 μM. (Green lines refer to the two tangent lines described in the text).</p>
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<p>I<sub>1</sub>/I<sub>3</sub> vs. polymer concentration plots for CAC determination regarding (<b>a</b>) H1 and (<b>b</b>) H2 copolymer aqueous solutions. (Green lines refer to the two tangent lines described in the text).</p>
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<p>TEM images from (<b>a</b>) P1 and (<b>b</b>) P2 copolymer solutions.</p>
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<p>TEM images from (<b>a</b>) H1 and (<b>b</b>) H2 copolymer solutions.</p>
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22 pages, 3631 KiB  
Article
Improving Atorvastatin Release from Polyelectrolyte Complex-Based Hydrogels Using Freeze-Drying: Formulation and Pharmaceutical Assessment of a Novel Delivery System for Oral Candidiasis Treatment
by Joanna Potaś-Stobiecka, Radosław Aleksander Wach, Bożena Rokita, Weronika Kaja Simonik, Magdalena Wróblewska, Karolina Borkowska, Silje Mork, Nataša Škalko-Basnet and Katarzyna Winnicka
Int. J. Mol. Sci. 2025, 26(5), 2267; https://doi.org/10.3390/ijms26052267 - 4 Mar 2025
Viewed by 195
Abstract
Atorvastatin calcium, an antifungal agent, has the potential to be repositioned/repurposed to combat the increasing antimicrobial resistance. However, one of the most crucial issues in developing atorvastatin calcium-loaded products with a topical antifungal effect is achieving the optimal release and dissolution rates of [...] Read more.
Atorvastatin calcium, an antifungal agent, has the potential to be repositioned/repurposed to combat the increasing antimicrobial resistance. However, one of the most crucial issues in developing atorvastatin calcium-loaded products with a topical antifungal effect is achieving the optimal release and dissolution rates of this statin to produce the desired therapeutic effect. In this paper, we report on the development and pharmaceutical assessment of hydrogels composed of low-molecular-weight chitosan, tragacanth, and xanthan gum/pectin/κ-carrageenan as potential drug carriers for atorvastatin calcium for buccal delivery. Multidirectional analysis of the carriers with regard to their drug-release profiles and mucoadhesive, antimicrobial, and cytotoxic properties was accompanied by an evaluation of the freeze-drying process used to improve the hydrogels’ applicability. Using differential scanning calorimetry, Fourier transform infrared spectroscopy, and scanning electron microscopy techniques, the role of lyophilization in enhancing atorvastatin calcium delivery from polyelectrolyte complex-based matrices via drug amorphization was demonstrated. The freeze-dried hydrogels had significantly improved release and dissolution rates for the amorphic statin. Therefore, there is great potential for the use of lyophilization in the design of polyelectrolyte complex-based semi-solids in usable dosage forms for numerous crystalline and poorly water-soluble active substances. Full article
(This article belongs to the Special Issue Applications of Biomaterials in Drug Development)
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Figure 1
<p>Mechanical properties of hydrogels H1–H3 and their placebo counterparts H1PL–H3PL (mean ± SD, n ≥ 5).</p>
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<p>In vitro ATC release from hydrogels H1–H3 with corresponding polynomial trend lines (mean ± SD, n = 3, <span class="html-italic">p</span> &lt; 0.05).</p>
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<p>In vitro ATC release from lyophilizates LH1–LH3 with corresponding polynomial trend lines (mean ± SD, n = 3, <span class="html-italic">p</span> &lt; 0.05).</p>
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<p>FTIR spectra of the drug-loaded and placebo lyophilizates in the wavelength range of 4000–500 cm<sup>−1</sup> (<b>A</b>), with a magnified view of the section between 1775 cm<sup>−1</sup> and 1425 cm<sup>−1</sup> (<b>B</b>).</p>
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<p>DSC thermograms (exothermic) obtained at first heating for ATC-loaded and placebo samples (<b>A</b>–<b>C</b>). Thermal behaviors of atorvastatin calcium (ATC) and LH1–LH3 and their respective physical mixtures (<b>D</b>–<b>F</b>). Cooling and second heating effects are presented in the figures included in the <a href="#app1-ijms-26-02267" class="html-app">Supplementary Materials (Figures S1–S7)</a>.</p>
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<p>Selected SEM images of the freeze-dried hydrogels (LH1–LH3 and LH1PL–LH3PL) under 100× (main pictures) and 1000× (magnified sections) magnification.</p>
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<p>Swelling behaviors of the hydrogels (<b>A</b>) and lyophilizates (<b>B</b>) in the simulated saliva solution (mean ± SD, n = 3).</p>
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<p>Mucoadhesive properties of the hydrogels (H1–H3, H1PL–H3PL), expressed as the (<b>A</b>) mucoadhesion force (F<sub>MAX</sub>, N) and (<b>B</b>) work of adhesion (W<sub>AD</sub>, µJ) (NC (negative control): cellulose paper; PC (positive control): Elugel<sup>®</sup>); mean ± SD, n ≥ 3.</p>
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<p>Mucoretention of the hydrogels (<b>A</b>) and lyophilizates (<b>B</b>) (PC (positive control): Elugel<sup>®</sup>); n = 3.</p>
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<p>Antimicrobial activities of the hydrogels (<b>A</b>) and lyophilizates (<b>B</b>) against <span class="html-italic">Candida albicans</span>, <span class="html-italic">C. krusei</span>, <span class="html-italic">C. parapsilosis</span>, and <span class="html-italic">Lactobacillus brevis</span> (controls: CLO cream with 1% (<span class="html-italic">w/w</span>) clotrimazole, ATC/DMSO, and ATC powder (atorvastatin calcium dissolved in DMSO or as a pure crystalline substance); mean ± SD, n = 3. The symbol “×” indicates no antimicrobial effect.</p>
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<p>Cell viability according to the modified (<b>A</b>) and standard MTT procedures (<b>B</b>) with respect to the positive (PC) and negative controls (NC: untreated cells). Cytotoxicity of the pure drug dissolved in DMSO (<b>C</b>). Mean cell viability ± SD, n = 8.</p>
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13 pages, 4814 KiB  
Article
Treatment of Sewage Sludge and Phosphorus Removal Using Polyacrylamide and Calcium Chloride
by Salam K. Al-Dawery, Yasmeen S. Al Hasani, Shafa D. Al Salimiya, Sajjala S. Reddy, Hanan A. Al Riyami, Hamed N. Harharah, Ramzi H. Harharah and Gasim Hayder
Water 2025, 17(5), 629; https://doi.org/10.3390/w17050629 - 21 Feb 2025
Viewed by 202
Abstract
The enhancement of the treatment of municipal wastewater treatment plants is limited by poor sludge settling qualities, and the excessive discharge of nitrogen and phosphorus exacerbate water eutrophication. The goal of the current work was to remove phosphorus from fresh sewage-activated sludge by [...] Read more.
The enhancement of the treatment of municipal wastewater treatment plants is limited by poor sludge settling qualities, and the excessive discharge of nitrogen and phosphorus exacerbate water eutrophication. The goal of the current work was to remove phosphorus from fresh sewage-activated sludge by developing a new conditioning and flocculation mechanism that included a coagulant and cationic polyelectrolytes in a dual conditioning system. The coagulant (CaCl2) and the high molecular weight polyacrylamide (CPAM-10) were chosen to be utilized singly or in pairs as cationic–coagulant combinations. The collected results showed that, in comparison to utilizing the coagulant (CaCl2), conditioning with the high molecular weight polymer (CPAM-10) produced improved settling and less turbidity. Only sludge with a lower solid content (TSS) exhibited better settling when pure CaCl2 was used for conditioning. CaCl2 conditioning enhanced settling by just 3%, while CPAM-10 improved the sludge setting by 60% for higher sludge TSSs. According to the results, conditioning settings using a dual mixture including 20 mL CPAM-10 and 50 mL CaCl2 improved settling by 80%. The amount of phosphorus in the supernatant was decreased by 15% and 9%, respectively, by using the coagulant (CaCl2) and 50 mL/L polyacrylamide (CPAM-10). As a result, there was a significant amount of phosphorus in the resultant supernatant. This suggested that the polymer had a significant impact on sludge settling because of its high positive charge, but had less of an impact on attracting phosphorus metal. Despite the lower positive charge of CaCl2, it has a dual action of settling and removing phosphorus. A considerable amount of phosphorus was removed from the sludge and leached to the supernatant during treatment. This treatment was coupled with less sludge settling. However, 90% phosphorus removal was achieved when mixed conditioning agents (20 mL CPAM-10 and 50 mL CaCl2) were used. Furthermore, phosphorus was reduced by 33 and 39%, respectively, by adding 20 milliliters of CaCl2 to 100 milliliters of the pre-conditioned supernatant with pure CPAM-10 and CaCl2. Using the CPAM-10 agent for sludge conditioning has a major impact on settling, because of the high positive charge, and because when a small amount of Ca++ is added to the polymer solution for conditioning to attract fine sludge particles and accelerate their combination, this results in flocculation and rapid dewatering. This mechanism allows for more phosphorus to be released to the supernatant, which has not been reported previously to the best of our knowledge. Full article
(This article belongs to the Section Wastewater Treatment and Reuse)
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Figure 1
<p>Shows a sample of sludge without conditioning.</p>
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<p>Sample treated with 100 mL CPAM-10 of a concentration of 1000 ppm.</p>
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<p>Sample treated with 100 mL CaCl<sub>2</sub> of a concentration of 1000 ppm.</p>
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<p>The settling after treatment with different concentrations.</p>
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<p>Sludge conditioning for different (TSSs) using 100 mL CaCl<sub>2</sub>; (<b>a</b>) percentage of settling improvement, (<b>b</b>) SVI.</p>
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<p>Sludge settling using pure CPAM-10.</p>
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<p>Sludge settling using pure CaCl<sub>2</sub>.</p>
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<p>Settling using a dual mixture of CaCl<sub>2</sub> and CPAM-10. (<b>a</b>) CaC<sub>2</sub> and 10 mL polymer, (<b>b</b>) CaC<sub>2</sub> and 20 mL polymer, (<b>c</b>) CaC<sub>2</sub> and 50 mL polymer.</p>
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<p>Phosphorus content in the supernatant after treatment with pure CaCl<sub>2</sub> and the polymer.</p>
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<p>Phosphorus removal from conditioned supernatant with pure CaCl<sub>2</sub> and CPAM-10.</p>
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<p>Phosphorus content in the supernatant after treatment using mixed CPAM-10 and different amounts of CaCl<sub>2</sub>.</p>
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22 pages, 3286 KiB  
Article
Background of New Measurement Electronic Devices with Polyelectrolyte Hydrogel Base
by Kaisarali Kadyrzhan, Ibragim Suleimenov, Lyazat Tolymbekova, Gaini Seitenova and Eldar Kopishev
Polymers 2025, 17(4), 539; https://doi.org/10.3390/polym17040539 - 19 Feb 2025
Viewed by 234
Abstract
It has been demonstrated that when a low-molecular-weight salt solution flows through a polyelectrolyte gel, an electromotive force is generated, and its polarity depends on the sign of the polyelectrolyte network’s charge. A mathematical model proving the possibility of developing a device for [...] Read more.
It has been demonstrated that when a low-molecular-weight salt solution flows through a polyelectrolyte gel, an electromotive force is generated, and its polarity depends on the sign of the polyelectrolyte network’s charge. A mathematical model proving the possibility of developing a device for separating a solution of low-molecular salt into enriched and depleted phases under the influence of gravitational forces has been developed. Such a device contains a system of parallel columns filled with different kinds of cross-linked polyelectrolyte networks. The proposed mathematical model is grounded in the theory of double electrical layers forming at the hydrogel/solution interface; these layers deform under non-equilibrium conditions, specifically during the flow of the solution through the cross-linked polyelectrolyte network. An analogous model is proposed describing the case of an analogous device based on an electric current passing through two oppositely charged contacting networks, which provides the possibility of separating the initial solution into enriched and the depleted phases too. The practical applications of the found effect are discussed. In particular, it is demonstrated that a wide number of measurement electronic devices can be created on such a base, including devices to be used within the investigation of polyelectrolyte hydrogels of different types. Full article
(This article belongs to the Section Polymer Networks)
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Figure 1

Figure 1
<p>Experimental setup for detecting the flow potential of a solution flowing through the hydrogel. The numbers represent the following: 1—hydrogel-filled tube (length: 50 mm, diameter: 20 mm); 2, 3—membranes separating the hydrogel from the low-molecular-weight salt solutions; 4—volume filled with a low-molecular-weight salt solution (height: 5 mm, volume: 10 mL); 5—buffer volume collecting the solution that passes through the hydrogel layer (volume: 50 mL); 6—electrodes for measuring the dynamic potential difference (sensitivity: millivolt range); and 7—precision voltmeter capable of measuring small voltage differences (accuracy: ±0.01 mV).</p>
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<p>Dependence of the observed electric potential difference above and below the hydrogel on the height of the solution column above the hydrogel, when the buffer volume is filled with water.</p>
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<p>The dependencies of the observed electrical potential difference above and below the hydrogel on the height of the solution column above the gel, when the buffer volume is filled with a solution of the same concentration as above the gel, were obtained from three independent experimental runs, and the standard deviations were determined.</p>
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<p>A variant of the diagram for separating the flow of low-molecular-weight salt into enriched and depleted. The numbers represent the following: 1—inlet for the feed solution of low-molecular-weight salt; 2, 3—column filled with a positively and negatively charged polyelectrolyte gel, respectively; 4—outlet for the depleted solution (salt concentration reduced); 5—outlet for the enriched solution (salt concentration increased); and 6, 7—auxiliary connecting elements facilitating the flow of the solution between the columns.</p>
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<p>Illustration of the effect of the redistribution of concentrations: (<b>a</b>)—dependence of the concentration of ionized functional groups, n, on the coordinate, (<b>b</b>)—dependence of the electric field magnitude E of the double electric layer on the coordinate, (<b>c</b>)—dependence of the electrostatic potential <math display="inline"><semantics> <mrow> <mi>φ</mi> </mrow> </semantics></math> on the coordinate, and (<b>d</b>)—dependence of the concentrations of the low-molecular ions of opposite signs n1 and n2 on the coordinate, the lower curve also corresponds to the behavior of the concentration of low-molecular salt [<a href="#B48-polymers-17-00539" class="html-bibr">48</a>].</p>
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<p>Formation of the analogue of the electrodialysis chamber in the considered system: <math display="inline"><semantics> <mrow> <msub> <mrow> <mi>E</mi> </mrow> <mrow> <mn>1</mn> </mrow> </msub> </mrow> </semantics></math>—the field generated due to the emergence of an electromotive force (EMF) caused by the flow of the solution through the polyelectrolyte networks; <math display="inline"><semantics> <mrow> <msub> <mrow> <mi>I</mi> </mrow> <mrow> <mn>1</mn> </mrow> </msub> </mrow> </semantics></math>—the flux of the initial solution; and <math display="inline"><semantics> <mrow> <msub> <mrow> <mi>I</mi> </mrow> <mrow> <mn>4</mn> </mrow> </msub> </mrow> </semantics></math>—the flux of the depleted solution.</p>
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<p>A modification of the scheme of <a href="#polymers-17-00539-f004" class="html-fig">Figure 4</a>: a transition to the direct contact of oppositely charged meshes. <math display="inline"><semantics> <mrow> <msub> <mrow> <mi>E</mi> </mrow> <mrow> <mn>2,3</mn> </mrow> </msub> </mrow> </semantics></math>—fields generated due to the emergence of an electromotive force (EMF) caused by the flow of the solution through polyelectrolyte networks; <math display="inline"><semantics> <mrow> <msub> <mrow> <mi>I</mi> </mrow> <mrow> <mn>1</mn> </mrow> </msub> </mrow> </semantics></math>—inflow of the initial solution; <math display="inline"><semantics> <mrow> <msub> <mrow> <mi>I</mi> </mrow> <mrow> <mn>4</mn> </mrow> </msub> </mrow> </semantics></math>—outflow of the depleted solution; and <math display="inline"><semantics> <mrow> <msub> <mrow> <mi>I</mi> </mrow> <mrow> <mn>2</mn> <mo>,</mo> <mn>3</mn> </mrow> </msub> </mrow> </semantics></math>—flows of the solution enriched with oppositely charged ions.</p>
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<p>The mechanism of formation of electric fields in the context of the scheme presented in <a href="#polymers-17-00539-f007" class="html-fig">Figure 7</a>: E<sub>2,3</sub>—fields arising due to the generation of an EMF caused by the flow of the solution through the polyelectrolyte networks; and E<sub>41,42</sub>—fields generated as a result of the solution flowing through the contact zone of oppositely charged networks.</p>
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<p>The anticipated configuration of the field within the contact zone of two oppositely charged networks. Bold circles highlight the schematic charges corresponding to the electric double layer formed through the contact of oppositely charged polyelectrolyte networks, while thin circles schematically indicate the charges corresponding to the double layers formed at the interface between the network and the solution.</p>
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<p>Modernized version of the scheme for the separation of the low-molecular-weight salt flow into enriched and depleted: 1—outlet for inflow of the initial solution of low-molecular salt into the system, 2—vessel filled with initial solution, 3—outlet for removal of depleted solution, 4—electrodes, 5—negatively charged network, 6—positively charged network, 7—vessel filled with depleted solution, and 8—outlet for depleted solution.</p>
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<p>Behavior of solutions for the linearized Equation (35) in the neighborhood of the contact region between oppositely charged meshes.</p>
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<p>A simplified representation of the electric field structure in the contact zone of oppositely charged meshes during the flow of electric current. Bold circles indicate schematic charges corresponding to the electric double layer formed at the contact point of oppositely charged polyelectrolyte networks, while thin circles schematically represent the charges associated with the double layers formed at the network–solution interface.</p>
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22 pages, 3684 KiB  
Review
Multilayered Polyelectrolyte Structures Deposited on Corona-Charged Substrate Blends as Potential Drug Delivery Systems
by Asya Viraneva, Maria Marudova, Aleksandar Grigorov, Sofia Milenkova and Temenuzhka Yovcheva
Coatings 2025, 15(2), 240; https://doi.org/10.3390/coatings15020240 - 18 Feb 2025
Viewed by 280
Abstract
Polyelectrolyte multilayers (PEMs) deposited on non-porous and porous blend substrates were studied. Films, prepared from two biodegradable polymers poly (D-lactic acid) (PDLA) and poly(ε-caprolactone) (PCL) and their blends were used as substrates in the present paper. All films were initially charged in a [...] Read more.
Polyelectrolyte multilayers (PEMs) deposited on non-porous and porous blend substrates were studied. Films, prepared from two biodegradable polymers poly (D-lactic acid) (PDLA) and poly(ε-caprolactone) (PCL) and their blends were used as substrates in the present paper. All films were initially charged in a corona discharge (positive or negative corona). After charging, the initial surface potential of the samples V0 was measured and the normalized surface potential was calculated. The dependencies on time of the normalized surface potential for electrets, possessing either positive or negative charges, were studied. It was found that the steady-state values of the normalized surface potential for the porous substrates were higher than those of the non-porous ones, independently of material type and corona polarity. It was also shown that the values of the normalized surface potential for the PCL electrets were the highest and decreased when the content of PDLA increased. Scanning electron microscopy (SEM) was utilized for the determination of the substrates’ surface morphology. With the largest pore size, PCL substrates allowed for a greater capture of charges on their surface and facilitated the retention of said charges for prolonged periods of time. Differential scanning calorimetry (DSC) measurements were performed to determine the degree of crystallinity, which was very high for PCL substrates, when compared to the other investigated substrates. The wettability of the investigated substrates was measured using the static water contact angle method. The obtained results demonstrated that the created blends were more hydrophilic than the pure films. The two chosen polyelectrolytes were layered onto the surface of the substrates with the use of the layer-by-layer (LbL) technique and benzydamine hydrochloride was loaded in the multilayers as a model drug. Its loading efficiency and release profile were carried out spectrophotometrically. It was determined that for non-porous substrates, independently of the corona polarity, the best fitting model was Korsmeyer-Peppas, while for the porous substrates the best fitting model was Weibull. Full article
(This article belongs to the Section Surface Coatings for Biomedicine and Bioengineering)
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<p>Corona discharge system: 1. high voltage source; 2. corona electrode; 3. grid; 4. grounded plate electrode; 5. sample on a metal pad; and 6. voltage divider.</p>
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<p>Schematic representation of the multilayer deposition process.</p>
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<p>Time dependencies of the normalized surface potential for PDLA substrates charged (<b>a</b>) in a positive corona and (<b>b</b>) in a negative corona.</p>
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<p>Time dependencies of the normalized surface potential for 50/50 substrates charged (<b>a</b>) in a positive corona and (<b>b</b>) in a negative corona.</p>
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<p>Time dependencies of the normalized surface potential for PCL substrates charged (<b>a</b>) in a positive corona and (<b>b</b>) in a negative corona.</p>
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<p>Steady-state values of the normalized surface potential at a time of 360 min for all investigated positively charged substrates.</p>
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<p>Steady-state values of the normalized surface potential at a time of 360 min for all investigated negatively charged substrates.</p>
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<p>SEM images of all investigated substrates.</p>
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<p>Surface free energy of all investigated substrates.</p>
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<p>Release profiles of Benzydamine Hydrochloride encapsulated in multilayer structures built on PDLA substrates treated with positive (+) or negative (−) corona.</p>
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<p>Release profiles of Benzydamine Hydrochloride encapsulated in multilayer structures built on substrates obtained from equal amounts of PDLA and PCL treated with positive (+) or negative (−) corona.</p>
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<p>Release profiles of benzydamine hydrochloride encapsulated in multilayer structures built on PCL substrates treated with positive (+) or negative (−) corona.</p>
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22 pages, 4582 KiB  
Article
Effect of Sequential vs. Simultaneous Dual Growth Factor Release from Structured Heparin-Poly-Electrolyte Multilayer Coatings on Peri-Implant Bone Formation and Angiogenesis in Pig Mandibles
by Philipp Kauffmann, Susanne Wolfer, Christina Behrens, Pauline Schlosser, Christian Dullin, Uwe Schirmer, Klaus Liefeith and Henning Schliephake
J. Funct. Biomater. 2025, 16(2), 67; https://doi.org/10.3390/jfb16020067 - 17 Feb 2025
Viewed by 291
Abstract
The aim of the present study was to test the sequential and simultaneous release of rhBMP2 and rhVEGF165 from poly-l-lysine-heparin (PLL-Hep) poly-electrolyte multilayer (PEM) coating on titanium surfaces for their ability to enhance peri-implant bone formation and CD31 expression around disc-shaped [...] Read more.
The aim of the present study was to test the sequential and simultaneous release of rhBMP2 and rhVEGF165 from poly-l-lysine-heparin (PLL-Hep) poly-electrolyte multilayer (PEM) coating on titanium surfaces for their ability to enhance peri-implant bone formation and CD31 expression around disc-shaped titanium implants (5 × 7 mm) in mini-pig mandibles. Bare titanium surfaces loaded with respective growth factor combinations served as controls. Ten different surface conditions were tested exhibiting early VEGF release, early BMP release, simultaneous VEGF and BMP release, and sole VEGF/BMP release, respectively. The implants were inserted press-fit into 5 mm trephine cavities at the lower border of the mandibles of mini-pigs and left to heal for 4 and 13 weeks. After 4 weeks, there was no significant difference in peri-implant bone formation, bone–implant contact nor CD31 expression between the different surface conditions. After 13 weeks, bone formation was significantly higher in the zone of 100 μm next to implant surfaces releasing either BMP alone or with an early release of BMP2. Expression of CD31 has significantly decreased from 4 to 13 weeks with significantly higher values in the group of implants with early release of BMP2. The results indicate that the range of released growth factors is limited to a distance of approximately 100 μm and that the sequence of early release of BMP2 followed by VEGF165 promotes peri-implant bone formation and peri-implant angiogenesis, which is in contrast to the current understanding of the temporal patterns of growth factor release for enhancement of bone formation. Full article
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<p>Clinical picture of implant insertion into the lower border of a mini pig mandible:.</p>
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<p>(<b>A</b>) Selection of the trephine defect for morphometric evaluation and (<b>B</b>) digitization of the bone area.</p>
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<p>(<b>A</b>): DAPI stain of nuclei in peri-implant tissue (blue); (<b>B</b>) Overlay of DAPI stain and CD31 expression (red); (<b>C</b>) Isolation of CD31-positive area; (<b>D</b>) Digitization of CD31-positive area.</p>
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<p>Micrographs of peri-implant bone formation: (<b>Top Row</b>): 4 weeks, (<b>Bottom Row</b>): 13 weeks, Bar: 2000 μm; (<b>A</b>) (PLL-Hep)<b><sub>10</sub></b> multilayer system loaded with rhBMP2 with a second (PLL-Hep)<sub>10</sub> multilayer system loaded with rhVGEF<sub>165</sub> on top; (<b>B</b>) (PLL-Hep)<sub>10</sub> multilayer system loaded with rhVGEF<sub>165</sub> with a second (PLL-Hep)<sub>10</sub> multilayer system loaded with rhBMP2 on top; (<b>C</b>) (PLL-Hep)<sub>20</sub> multilayer system simultaneously loaded with rhVGEF<sub>165</sub> and rhBMP2; (<b>D</b>) (PLL-Hep)<sub>20</sub> multilayer system loaded with rhVGEF<sub>165</sub> only; (<b>E</b>) (PLL-Hep)<sub>20</sub> multilayer system loaded with rhBMP2 only; (<b>F</b>) (PLL-Hep)<sub>20</sub> multilayer system without growth factor loading (control); (<b>G</b>) Ti surface loaded simultaneously loaded with rhVGEF<sub>165</sub> and rhBMP2; (<b>H</b>) Ti surface loaded with rhVGEF<sub>165</sub> only; (<b>I</b>) Ti surface loaded with rhBMP2 only; (<b>J</b>): Ti surface unloaded (control).</p>
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<p>Bone area (mm<sup>2</sup>) and bone density (%) of newly formed bone within the trephine defects. Data are presented as means ± standard deviation (SD) with <span class="html-italic">n</span> = 6.</p>
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<p>Bone area (mm<sup>2</sup>) of newly formed bone within the peri-implant zone (300 μm). Data are presented as means ± standard deviation (SD) with <span class="html-italic">n</span> = 6; (*): significantly different from Ti control surface (<span class="html-italic">p</span> ≤ 0.05).</p>
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<p>Bone area (mm<sup>2</sup>) of newly formed bone within the immediate surface layer (100 μm). Data are presented as means ± standard deviation (SD) with <span class="html-italic">n</span> = 6. (*): significantly different from Ti control surface (<span class="html-italic">p</span> ≤ 0.05).</p>
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<p>Bone–implant contact (%); data are presented as means ± standard deviation (SD) with <span class="html-italic">n</span> = 6; (*): significantly different from Ti control surface (<span class="html-italic">p</span> &lt; 0.05); <sup>‡</sup>: significantly higher than PEM coating with the 2-zone architecture with VEGF in the upper zone and BMP below as well as PEM coating with VEGF loading only (<span class="html-italic">p</span> &lt;&lt; 0.05); (<b><sup>§</sup></b>): significantly different from PEM-coated unloaded surface (<span class="html-italic">p</span> &lt; 0.05).</p>
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<p>Overview of CD31-positive expression after 4 weeks (bar = 100 μm); (<b>A</b>) (PLL-Hep)<b><sub>10</sub></b> multilayer system loaded with rhBMP2 with a second (PLL-Hep)<sub>10</sub> multilayer system loaded with rhVGEF<sub>165</sub> on top; (<b>B</b>) (PLL-Hep)<b><sub>10</sub></b> multilayer system loaded with rhVGEF<sub>165</sub> with a second (PLL-Hep)<sub>10</sub> multilayer system loaded with rhBMP2 on top; (<b>C</b>) (PLL-Hep)<sub>20</sub> multilayer system simultaneously loaded with rhVGEF<sub>165</sub> and rhBMP2; (<b>D</b>) Ti surface loaded simultaneously loaded with rhVGEF<sub>165</sub> and rhBMP2; (<b>E</b>) Ti surface loaded with rhBMP2 only; (<b>F</b>) Ti surface unloaded (control).</p>
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<p>Overview of CD31-positive expression after 13 weeks (bar = 100 μm); (<b>A</b>) (PLL-Hep)<b><sub>10</sub></b> multilayer system loaded with rhBMP2 with a second (PLL-Hep)<sub>10</sub> multilayer system loaded with rhVGEF<sub>165</sub> on top; (<b>B</b>) (PLL-Hep)<b><sub>10</sub></b> multilayer system loaded with rhVGEF<sub>165</sub> with a second (PLL-Hep)<sub>10</sub> multilayer system loaded with rhBMP2 on top; (<b>C</b>) (PLL-Hep)<b><sub>20</sub></b> multilayer system simultaneously loaded with rhVGEF<sub>165</sub> and rhBMP2; (<b>D</b>) Ti surface loaded simultaneously loaded with rhVGEF<sub>165</sub> and rhBMP2; (<b>E</b>) Ti surface loaded with rhBMP2 only; (<b>F</b>) Ti surface unloaded (control).</p>
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<p>Area of CD31-positive expression (μm<sup>2</sup>/10<sup>3</sup>); data are presented as means ± standard deviation (SD) with n = 6.</p>
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24 pages, 5579 KiB  
Article
Uptake and Inhibition of P-Glycoprotein-Mediated Efflux Evaluation of Encapsulated Methotrexate Chitosan and Hypromellose Phthalate Nanoparticles for Potential Glioblastoma Treatment
by Valéria de Moura Leite Naves, Rafaela Franco Dias Bruzadelli, Marisa Ionta, Maria Palmira Daflon Gremião, Liliane Neves Pedreiro, Gislaine Ribeiro Pereira and Flávia Chiva Carvalho
Pharmaceutics 2025, 17(2), 239; https://doi.org/10.3390/pharmaceutics17020239 - 12 Feb 2025
Viewed by 468
Abstract
Background: Methotrexate (MTX), a folic acid antagonist used in chemotherapy, faces limitations due to cancer cell resistance, high toxicity, and low bioavailability. Objective: This study developed nanoparticles (NPs) of chitosan (QS) and hydroxypropylmethylcellulose phthalate (HPMCP) to encapsulate MTX for potential effect investigation on [...] Read more.
Background: Methotrexate (MTX), a folic acid antagonist used in chemotherapy, faces limitations due to cancer cell resistance, high toxicity, and low bioavailability. Objective: This study developed nanoparticles (NPs) of chitosan (QS) and hydroxypropylmethylcellulose phthalate (HPMCP) to encapsulate MTX for potential effect investigation on glioblastoma cell targeting and P-gp efflux inhibition. Method: NPs were produced by the polyelectrolyte complexation method and were characterized by DLS, PDI, DSC, FTIR, PXRD, MEV, drug release profile, and an in vitro mucoadhesion test. Cell viability, flow cytometry, and LSCM using U251MG (glioblastoma) and CCD 1059Sk (fibroblasts) cells were used to evaluate glioblastoma and the P-gp efflux effect. Results: NPPM29 (QS3:1) showed 91.72% encapsulation efficiency, a mean diameter of 452.6 nm, and a zeta potential of +22.5 mV. DSC, FTIR, and PXRD confirmed the QS-HPMCP supramolecular interaction. Liquid falling mucoadhesion tests demonstrated strong retention of NPPM29 (84%) compared to free MTX (10.5%). In vitro release studies indicated controlled drug release at pH 7.4. Cytotoxicity assays in U251MG revealed enhanced efficacy of NPPM29 (IC50 = 68.79 µg/mL) compared to free MTX (IC50 = 80.54 µg/mL), with minimal impact on fibroblasts, confirming tumor specificity. Flow cytometry and LSCM confirmed improved cellular internalization and P-gp inhibition. Conclusions: These findings highlight the potential of MTX-QS-HPMCP-NPs for glioblastoma therapy. Full article
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<p>SEM microphotograph of NPPM29 at 32,830× (<b>top</b>) and 20,000× (<b>bottom</b>).</p>
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<p>X-ray diffraction spectrum of the drug and polymers and NPPM29 and NPTM33.</p>
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<p>TGA and DTA curves of QS (<b>A</b>), MTX (<b>B</b>), and QS compared to NPPM29 (<b>C</b>) obtained in the 25 °C range at 1100 °C, under a nitrogen atmosphere and heating rates of 20 °C.min<sup>−1</sup>.</p>
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<p>DSC curves of methotrexate (MTX), nanoparticles (NPP29, NPPM29, NPT33, NPTM33), and polymers (chitosan, HPMCP, and TPP).</p>
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<p>NanoDSC curves of methotrexate (MTX), nanoparticles (NPP29, NPPM29, NPT33, NPTM33), and polymers (chitosan, HPMCP, and TPP).</p>
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<p>Adsorbed mucin on nanoparticles related to the amount of added mucin.</p>
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<p>Drug release profile of NPTM33, NPPM29, and MTX solution in acidic (<b>A</b>) and neutral environments (<b>B</b>). The lines indicate the fit of the Korsmeyer–Peppas and Weibull kinetic models.</p>
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<p>Relative cell viability of U251MG glioblastoma cells determined by MTS assay. (NPP29) CS/HPMCP nanoparticles, (NPPM29) CS/HPMCP/MTX nanoparticles, (NPTM33) CS/TPP/MTX nanoparticles, and MTX (Methotrexate). (***) <span class="html-italic">p</span> value ˂ 0.001 according to ANOVA followed by Dunnet’s post-test.</p>
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<p>Relative cell viability of primary skin fibroblasts (CCD-1059Sk) determined by MTS assay. (NPP29) QS/HPMCP NPs, (NPPM29) QS/HPMCP/MTX NPs, (NPTM33) QS/TPP/MTX NPs, and MTX (Methotrexate). (***) <span class="html-italic">p</span> value ≤ 0.001 according to ANOVA followed by Dunnet’s post-test.</p>
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<p>Incorporation profile of NPP29 (QS-FITC) by U251MG cells, derived from glioblastoma, by flow cytometry and fluorescence microscopy. In (<b>top</b>, <b>left</b>) flow cytometry analysis of control cells (not exposed to NPP29); (<b>top</b>, <b>right</b>) flow cytometry analysis of cells exposed to NPP29 for 24 h; (<b>bottom</b>) illustrative image obtained by fluorescence microscopy (400×) evidencing positive cells, which internalized the NPP29 (QS-FITC, green). The cell nuclei were marked with DAPI and are evidenced in blue.</p>
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<p>Flow cytometry results of glioblastoma cells incubated with MTX/FITC and NPPM29 for 2 h (<b>left</b>) and 6 h (<b>right</b>) exposure. Fluorescence intensity profiles: red population: exposed to culture medium only (negative control), yellow population: exposed to MTX-FITC, green population: exposed to NP-FITC.</p>
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<p>Flow cytometry analysis on U251MG cells, derived from glioblastoma, exposed to MTX/FITC (orange), MTX/FITC-QS (green), MTX/FITC-HPMCP (light blue), and NPPM29 (pink) for 12 h (<b>left</b>) and 24 h (<b>right</b>). Fluorescence intensity profiles: The red range represents the population exposed only to the culture medium, thus without fluorescence (negative control).</p>
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<p>Flow cytometry analysis of U251MG glioblastoma cells exposed to MTX/FITC (green), NPPM29 (orange), MTX/FITC-verapamil (10 µM) (dark blue), and NPPM29-verapamil (10 µM) (light blue) for 24 h. The red interval represents the population exposed only to the culture medium, without fluorescence (negative control).</p>
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<p>Three-dimensional Images Generated by Confocal Microscopy of NPPM29 Inside Tumor Cells After 12 h (<b>bottom-left</b>) and 24 h (<b>bottom-right</b>) of Treatment. Cells without treatment as control (<b>top</b>). The green fluorescence corresponds to the FITC in the NPs.</p>
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23 pages, 6806 KiB  
Article
Synthesis and Characterization of Innovative Double-Network Hydrogels with Potential as Adsorbent Materials for Wastewater Treatment
by Alexandra Vieru, Onur Yilmaz, Alina Gabriela Rusu, Cătălina Natalia Yilmaz, Alina Ghilan and Loredana Elena Nita
Polymers 2025, 17(4), 463; https://doi.org/10.3390/polym17040463 - 10 Feb 2025
Viewed by 539
Abstract
Nowadays, large amounts of wastewater arise from various industrial applications. The discharge of wastewater into the environment represents a threat to the aquatic ecosystem and human health. Thus, in the present study, innovative double-network (DN) hydrogels with pH-sensitive features and applicability as adsorbents [...] Read more.
Nowadays, large amounts of wastewater arise from various industrial applications. The discharge of wastewater into the environment represents a threat to the aquatic ecosystem and human health. Thus, in the present study, innovative double-network (DN) hydrogels with pH-sensitive features and applicability as adsorbents in the treatment of leather dye wastewater were prepared. The polyelectrolyte, poly(N,N-dimethylaminoethyl methacrylate (PDMAEMA), was obtained via the radical polymerization process, while the supramolecular structure was co-assembled through physical interactions. As a novelty, the double network was obtained through the interpenetration of the supramolecular network in the cross-linked polymeric one. The new hydrogels were physico-chemically and morphologically characterized by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and in terms of thermogravimetric analysis (TGA), swelling degree measurements, and dye adsorption studies. The DN hydrogels present interconnected macropores and high thermal stability. The swelling capacity of the dual network gels highlights a superadsorbent behavior at pH 3. Furthermore, the dye adsorption study highlights the effects of several variables (pH, concentration dose of adsorbent) on the ability of the gels to adsorb an anionic dye. The adsorption kinetics of the anionic dyes fitted the pseudo-first-order model (PFO). The estimated maximum adsorption capacities for the anionic dyes was 451 mg g−1 for PDMAEMA and 545 mg g−1 for DN gel. Full article
(This article belongs to the Special Issue Functional Gel and Their Multipurpose Applications)
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<p>Schematic representation of the PDMAEMA-based synthetic network.</p>
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<p>Schematic representation of the supramolecular network formation.</p>
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<p>Schematic representation of the hybrid double-network formation.</p>
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<p>FTIR spectra of (<b>a</b>) the S<sub>1</sub> supramolecular system co-assembled in 1:1 and 1:3 ratio, and (<b>b</b>) PDMAEMA and DN gels.</p>
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<p>TGA graphs of the PDMAEMA network and PDMAEMA_(S<sub>1</sub> 1:3) DN gel.</p>
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<p>SEM images of the S<sub>1</sub> supramolecular structure co-assembled in 1:1 and 1:3 ratios, PDMAEMA gel, and the DN gels.</p>
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<p>Pore size distribution histograms for PDMAEMA and PDMAEMA_(S1 1:3).</p>
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<p>The equilibrium swelling degree of the PDMAEMA and PDMAEMA_(S<sub>1</sub> 1:3) DN at different pHs.</p>
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<p>The dye adsorption capacity as a function of adsorbent dose.</p>
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<p>Adsorption capacity of PDMAEMA_(S<sub>1</sub> 1:3) as a function of pH.</p>
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<p>The appearance of dye solution over time as a function of the absorption ability of PDMAEMA_(S<sub>1</sub> 1:3).</p>
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<p>The dye removal efficiency of PDMAEMA and PDMAEMA_(S<sub>1</sub> 1:3) in time.</p>
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<p>The dye adsorption capacity of PDMAEMA and PDMAEMA_(S<sub>1</sub> 1:3) with variation in dye concentration.</p>
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<p>The reuse capacity of the studied materials for anionic dye.</p>
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<p>SellaSet Blue HN dye adsorption kinetic data fitted into the PFO model.</p>
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<p>SellaSet Blue HN dye adsorption kinetic data fitted into the PSO model.</p>
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<p>SellaSet Blue HN dye adsorption kinetic data fitted into the IPD.</p>
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25 pages, 5193 KiB  
Article
Polyelectrolyte Complex Dry Powder Formulations of Tobramycin with Hyaluronic Acid and Sodium Hyaluronate for Inhalation Therapy in Cystic Fibrosis-Associated Infections
by Yanina de Lafuente, Eride Quarta, María S. Magi, Ana L. Apas, Joaquín Pagani, María C. Palena, Paulina L. Páez, Fabio Sonvico and Alvaro F. Jimenez-Kairuz
Antibiotics 2025, 14(2), 169; https://doi.org/10.3390/antibiotics14020169 - 8 Feb 2025
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Abstract
Background/Objectives: Pulmonary delivered tobramycin (TOB) is a standard treatment for Pseudomonas aeruginosa lung infections, that, along with Staphylococcus aureus, is one of the most common bacteria causing recurring infections in CF patients. However, the only available formulation on the market containing tobramycin, TOBI [...] Read more.
Background/Objectives: Pulmonary delivered tobramycin (TOB) is a standard treatment for Pseudomonas aeruginosa lung infections, that, along with Staphylococcus aureus, is one of the most common bacteria causing recurring infections in CF patients. However, the only available formulation on the market containing tobramycin, TOBI®, is sold at a price that makes the access to the treatment difficult. Therefore, this work focuses on the development and characterization of an ionic complex between a polyelectrolyte, hyaluronic acid (HA) and its salt, sodium hyaluronate (NaHA), and TOB to be formulated as an inhalable dry powder. Methods: The solid state complex obtained by spray drying technique was physicochemically characterized by infrared spectroscopy, thermal analysis and X-ray diffraction, confirming an ionic interaction for both complexes. Results: The powder density, geometric size, and morphology along with the aerodynamic performance showed suitable properties for the powder formulations to reach the deep lung. Moisture uptake was found to be low, with the complex HA-TOB remaining physicochemically unchanged, while the NaHA-TOB required significant protection against humidity. The biopharmaceutical in vitro experiments showed a rapid dissolution which can have a positively impact in reducing side effects, while the drug release study demonstrated a reversible polyelectrolyte–drug interaction. Microbiological experiments against P. aeruginosa and S. aureus showed improved bacterial growth inhibition and bactericidal efficacy, as well as better inhibition and eradication of biofilms when compared with to TOB. Conclusions: A simple polyelectrolyte-drug complex technique represents a promising strategy for the development of antimicrobial dry powder formulations for pulmonary delivery in the treatment of cystic fibrosis (CF) lung infections. Full article
(This article belongs to the Section Antibiotics Use and Antimicrobial Stewardship)
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<p>Overlapped Fourier transform infrared spectroscopy spectra of HA-TOB and NaHA-TOB complexes; raw materials (tobramycin (TOB), hyaluronic acid (HA), and sodium hyaluronate (NaHA)) and physical mixtures (PM) of both complexes.</p>
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<p>Thermal analysis by differential scanning calorimetry (DSC) (<b>a</b>) and thermogravimetric analysis (TGA) (<b>b</b>) of the complex HA-TOB, its raw materials, and the physical mixture (PM). DSC (<b>c</b>) and TGA (<b>d</b>) of the complex NaHA-TOB, its raw materials, and the PM.</p>
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<p>Powder X-ray diffraction patterns of the HA-TOB, its precursors, and its PM (<b>A</b>) and of the NaHA-TOB, its raw materials, and its PM (<b>B</b>).</p>
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<p>Scanning electron microscopy (SEM) micrographs of TOB (<b>a</b>), HA-TOB (<b>b</b>), and NaHA-TOB (<b>c</b>) obtained by spray drying with magnifications of 500×, 1000×, 5000×, and 10,000×. The arrows indicate the deposition on the particles of crystalline non-complexed TOB.</p>
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<p>Moisture uptake of the complexes stored at 25 °C and a relative humidity (RH) of 31 and 76 (<b>a</b>). SEM micrographs of HA-TOB at a magnification of 1000× (<b>b</b>) and 5000× (<b>c</b>), and NaHA-TOB at a magnification of 1000× (<b>d</b>) after storage at 25 °C and 76% HR in a sealed container.</p>
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<p>TOB deposited and recovered from the inhaler device and capsule, and the different stages of the NGI of the HA-TOB and NaHA-TOB.</p>
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<p>Dissolution profiles of the complexes HA-TOB and NaHA-TOB, and the drug (TOB).</p>
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<p>SEM micrographs at a magnification of 1000× (1) and 5000× (2) of the biofilm produced by <span class="html-italic">P. aeruginosa</span> and <span class="html-italic">S. aureus</span> not treated (<b>A1</b>,<b>A2</b>) and treated with HA-TOB to evaluate the inhibition (<b>B1</b>,<b>B2</b>) and eradication (<b>C1</b>,<b>C2</b>) of the respective strains.</p>
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20 pages, 2441 KiB  
Article
An Investigation into the Factors Influencing the Effectiveness of a Biodegradable Natural Coagulant Derived from Phaseolus vulgaris Seeds and Coagulation Mechanism
by Jelena M. Prodanović, Nataša M. Nastić, Marina B. Šćiban, Dragana V. Lukić, Vesna M. Vasić and Nevena T. Blagojev
Sustainability 2025, 17(4), 1372; https://doi.org/10.3390/su17041372 - 7 Feb 2025
Viewed by 443
Abstract
One of the major criteria for monitoring water and wastewater quality is turbidity, which is most often reduced using chemical coagulants and flocculants, such as alum and iron salts and acrylamide. However, due to their detrimental effects, intensive investigations into natural coagulants and [...] Read more.
One of the major criteria for monitoring water and wastewater quality is turbidity, which is most often reduced using chemical coagulants and flocculants, such as alum and iron salts and acrylamide. However, due to their detrimental effects, intensive investigations into natural coagulants and flocculants have recently been conducted. These coagulants are biodegradable, derived from renewable sources, and do not pose health risks, making them a sustainable solution for water and wastewater treatment. Coagulation and flocculation using natural coagulants is a complex phenomenon influenced by multiple factors. In this study, the impact of the solvent used to extract the natural coagulant from Phaseolus vulgaris seeds on its coagulation effectiveness was examined, along with the effects of pH, the initial turbidity of the treated water, and the applied coagulant dose. The extract obtained using 0.5 mol/L NaCl demonstrated higher coagulation activity compared to the extract obtained with distilled water. Both extracts exhibited improved performance in water with higher initial turbidity (200 NTU) and at the lowest pH tested (pH 6). Under these conditions, the water extract achieved a maximum coagulation activity of 58.4% at a dose of 0.1 mL/L, while the NaCl extract reached an 83.5% turbidity reduction at a dose of 0.4 mL/L. The dominant coagulants in the NaCl extract of Phaseolus vulgaris seeds are anionic polyelectrolytes. In the presence of divalent cations, these coagulants destabilize negatively charged particles through either the bridging mechanism or the sweep coagulation mechanism. Full article
(This article belongs to the Section Environmental Sustainability and Applications)
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<p>The effect of the applied doses of the water extract from common bean on coagulation activity in model waters with varying initial turbidities and pH values: (<b>a</b>) pH 6, (<b>b</b>) pH 8, and (<b>c</b>) pH 10.</p>
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<p>The effect of the applied doses of the water extract from common bean on coagulation activity in model waters with varying initial turbidities and pH values: (<b>a</b>) pH 6, (<b>b</b>) pH 8, and (<b>c</b>) pH 10.</p>
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<p>The effect of the applied doses of the NaCl extract from common bean on coagulation activity in model waters with varying initial turbidities and pH values: (<b>a</b>) pH 6, (<b>b</b>) pH 8, and (<b>c</b>) pH 10.</p>
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<p>The effect of the applied doses of the NaCl extract from common bean on coagulation activity in model waters with varying initial turbidities and pH values: (<b>a</b>) pH 6, (<b>b</b>) pH 8, and (<b>c</b>) pH 10.</p>
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<p>The effect of pH on the coagulation activity of the water extract from common bean in model waters with varying initial turbidities: (<b>a</b>) 50 NTU, (<b>b</b>) 100 NTU, and (<b>c</b>) 200 NTU.</p>
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<p>The effect of pH on the coagulation activity of the water extract from common bean in model waters with varying initial turbidities: (<b>a</b>) 50 NTU, (<b>b</b>) 100 NTU, and (<b>c</b>) 200 NTU.</p>
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<p>The effect of pH on the coagulation activity of the NaCl extract from common bean in model waters with varying initial turbidities: (<b>a</b>) 50 NTU, (<b>b</b>) 100 NTU, and (<b>c</b>) 200 NTU.</p>
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<p>The effect of the concentration of CaCl<sub>2</sub> on the coagulation activity of the NaCl extract from common bean in model waters with initial turbidity 220 NTU and pH 5.5 and 11.</p>
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<p>The effect of the concentration of CaSO<sub>4</sub> on the coagulation activity of the NaCl extract from common bean in model waters with initial turbidity 220 NTU and pH 5.5 and 11.</p>
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<p>The effect of the concentration of MgSO<sub>4</sub> on the coagulation activity of the NaCl extract from common bean in model waters with initial turbidity 220 NTU and pH 5.5 and 11.</p>
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<p>The effect of the concentration of NaCl on the coagulation activity of the NaCl extract from common bean in model waters with initial turbidity 220 NTU and pH 5.5 and 11.</p>
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11 pages, 2190 KiB  
Article
Transient Electroosmosis on a Soft Surface
by Hiroyuki Ohshima
Colloids Interfaces 2025, 9(1), 12; https://doi.org/10.3390/colloids9010012 - 4 Feb 2025
Viewed by 690
Abstract
A general theory was developed for the time-dependent transient electroosmosis on a planar soft surface, i.e., a polyelectrolyte-coated solid surface in an electrolyte solution, when an electric field is suddenly applied. This serves as a simple model for the time-dependent electrokinetic phenomena occurring [...] Read more.
A general theory was developed for the time-dependent transient electroosmosis on a planar soft surface, i.e., a polyelectrolyte-coated solid surface in an electrolyte solution, when an electric field is suddenly applied. This serves as a simple model for the time-dependent electrokinetic phenomena occurring at biointerfaces. A closed-form approximate expression is derived for the electroosmotic velocity distribution within the polyelectrolyte layer as a function of both position and time. This analysis reveals that the temporal and spatial variations in the electroosmotic flow caused by the surface charges of the solid surface is confined to the region near the solid surface. In contrast, the variations due to the fixed charges within the polyelectrolyte layer extend over a wider region inside the polyelectrolyte layer. Full article
(This article belongs to the Special Issue Biocolloids and Biointerfaces: 2nd Edition)
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Figure 1

Figure 1
<p>Transient electroosmotic flow with velocity <span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) on a soft surface, that is, a charged solid surface with a surface charge density <span class="html-italic">σ</span>, covered by a polyelectrolyte layer of thickness <span class="html-italic">D</span> and volume charge density <span class="html-italic">ρ</span><sub>fix</sub>, immersed in an electrolyte solution in response to an applied electric field <span class="html-italic">E</span>(<span class="html-italic">t</span>). The thickness <span class="html-italic">D</span> of the polyelectrolyte layer is much larger than both the Debye length 1/<span class="html-italic">κ</span> and the Brinkmann screening length 1/<span class="html-italic">λ</span>, so that the thickness <span class="html-italic">D</span> can be practically regarded as infinite.</p>
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<p>The temporal and spatial variations in the <span class="html-italic">z</span>-component <span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) of the electroosmotic flow velocity <span class="html-italic">u</span><sub>1</sub>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) caused by the fixed charges in the polyelectrolyte layer with a surface charge density <span class="html-italic">σ</span><sub>.</sub> The 3D plot of the scaled electroosmotic velocity defined by <span class="html-italic">u</span><sub>1</sub>*(<span class="html-italic">x</span>, <span class="html-italic">t</span>) = −<span class="html-italic">u</span><sub>1</sub>(<span class="html-italic">x</span>, <span class="html-italic">t</span>)/(<span class="html-italic">σE</span>/<span class="html-italic">ηκ</span>) is plotted as a function of the scaled distance <span class="html-italic">κx</span> from the solid surface and the scaled time <span class="html-italic">κ</span><sup>2</sup><span class="html-italic">νt</span>, calculated using Equation (21) for the case of <span class="html-italic">λ</span>/<span class="html-italic">κ</span> = 0.5. Here, the minus sign indicates that the electroosmotic flow occurs in the direction opposite to that of the applied electric field <span class="html-italic">E</span>(<span class="html-italic">t</span>).</p>
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<p>The temporal and spatial variations in the <span class="html-italic">z</span>-component <span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) of the electroosmotic flow velocity <span class="html-italic">u</span><sub>2</sub>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) caused by the fixed charges in the polyelectrolyte layer with a volume charge density <span class="html-italic">ρ</span><sub>fix.</sub> The 3D plot of the scaled electroosmotic velocity defined by <span class="html-italic">u</span><sub>2</sub>*(<span class="html-italic">x</span>, <span class="html-italic">t</span>) = −<span class="html-italic">u</span><sub>2</sub>(<span class="html-italic">x</span>, <span class="html-italic">t</span>)/(<span class="html-italic">ρ</span><sub>fix.</sub>/<span class="html-italic">ηλ</span><sup>2</sup>) is plotted as a function of the reduced distance <span class="html-italic">λx</span> from the solid surface and the scaled time <span class="html-italic">λ</span><sup>2</sup><span class="html-italic">νt</span>, calculated using Equation (22).</p>
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<p>The temporal and spatial variations in the <span class="html-italic">z</span>-component <span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) of the electroosmotic flow velocity <span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) caused by the fixed charges in the polyelectrolyte layer with a volume charge density <span class="html-italic">ρ</span><sub>fix.</sub> The 3D plot of the scaled electroosmotic velocity defined by <span class="html-italic">u</span>*(<span class="html-italic">x</span>, <span class="html-italic">t</span>) = −<span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>)/(<span class="html-italic">ρ</span><sub>fix.</sub>/<span class="html-italic">ηλ</span><sup>2</sup>) is plotted as a function of the reduced distance <span class="html-italic">λx</span> from the solid surface and the scaled time <span class="html-italic">λ</span><sup>2</sup><span class="html-italic">νt</span>, using Equations (20)–(22) for the case where <span class="html-italic">λ</span>/<span class="html-italic">κ</span> = 0.5 and <span class="html-italic">κρ</span><sub>fix</sub>/<span class="html-italic">λ</span><sup>2</sup><span class="html-italic">σ</span> = 0.4.</p>
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<p>The temporal and spatial variations in the <span class="html-italic">z</span>-component <span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) of the electroosmotic flow velocity <span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) caused by the fixed charges in the polyelectrolyte layer with a volume charge density <span class="html-italic">ρ</span><sub>fix.</sub> The 3D plot of the scaled electroosmotic velocity defined by <span class="html-italic">u*</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>) = −<span class="html-italic">u</span>(<span class="html-italic">x</span>, <span class="html-italic">t</span>)/(<span class="html-italic">ρ</span><sub>fix.</sub>/<span class="html-italic">ηλ</span><sup>2</sup>) is plotted as a function of the reduced distance <span class="html-italic">λx</span> from the solid surface and the scaled time <span class="html-italic">λ</span><sup>2</sup><span class="html-italic">νt</span>, using Equations (20)–(22) for the case where <span class="html-italic">λ</span>/<span class="html-italic">κ</span> = 0.5 and <span class="html-italic">κρ</span><sub>fix</sub>/<span class="html-italic">λ</span><sup>2</sup><span class="html-italic">σ</span> = −0.4.</p>
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12 pages, 2055 KiB  
Article
Effect of Ammonium Salt on Conjugated Polyelectrolyte as an Interlayer for Organic–Inorganic Hybrid Perovskite Memristors
by Eun Soo Shim, Ji Hyeon Lee, Ju Wan Park, Sun Woo Kim, Su Bin Park and Jea Woong Jo
Nanomaterials 2025, 15(3), 227; https://doi.org/10.3390/nano15030227 - 30 Jan 2025
Viewed by 648
Abstract
Memristors are promising candidates for next-generation non-volatile memory devices, offering low power consumption and high-speed switching capabilities. However, conventional metal oxide-based memristors are constrained by fabrication complexity and high costs, limiting their commercial viability. Organic–inorganic hybrid perovskites (OIHPs), known for their facile solution [...] Read more.
Memristors are promising candidates for next-generation non-volatile memory devices, offering low power consumption and high-speed switching capabilities. However, conventional metal oxide-based memristors are constrained by fabrication complexity and high costs, limiting their commercial viability. Organic–inorganic hybrid perovskites (OIHPs), known for their facile solution processability and unique ionic–electronic conductivity, provide an attractive alternative. This study presents a conjugated polyelectrolyte (CPE), PhNa-1T, as an interlayer for OIHP memristors to enhance the high-resistance state (HRS) performance. A post-treatment process using n-octylammonium bromide (OABr) was further applied to optimize the interlayer properties. Devices treated with PhNa-1T/OABr achieved a significantly improved ON/OFF ratio of 2150, compared to 197 for untreated devices. Systematic characterization revealed that OABr treatment improved film morphology, reduced crystallite strain, and optimized energy level alignment, thereby reinforcing the Schottky barrier and minimizing current leakage. These findings highlight the potential of tailored interlayer engineering to improve OIHP-based memristor performance, offering promising prospects for applications in non-volatile memory technologies. Full article
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Graphical abstract

Graphical abstract
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<p>(<b>a</b>) Chemical structure of PhNa−1T and OABr. (<b>b</b>) UV−Vis absorbance spectra of PhNa−1T and PhNa−1T/OABr. (<b>c</b>) XPS plots of S 2p for PhNa−1T films before and after OABr treatment (dotted points are raw data, and blue lines are total fitted data, yellow lines are S 2<span class="html-italic">p</span><sub>1/2</sub> for SO<sub>3</sub><sup>−</sup>, red lines are S 2<span class="html-italic">p</span><sub>3/2</sub> for SO<sub>3</sub><sup>−</sup>, peach lines are S 2<span class="html-italic">p</span><sub>1/2</sub> for S, and green lines are S 2<span class="html-italic">p</span><sub>3/2</sub> for S). (<b>d</b>) Memristic <span class="html-italic">I−V</span> curve of PhNa−1T interlayer with OIHP (inset image: device architecture).</p>
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<p>(<b>a</b>) Schematic device configuration of the OHP memristor used in this study. (<b>b</b>) Current–voltage measurement of the memristors with PhNa−1T and PhNa−1T/OABr interlayers. (<b>c</b>) Endurance and (<b>d</b>) retention testing results for OIHP memristors depending on interlayers (Resistance range at HRS were shaded with color for retention tests).</p>
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<p>(<b>a</b>) AFM images and (<b>b</b>) XRD patterns for the PbBr<sub>2</sub> films on PhNa−1T and PhNa−1T/OABr. (<b>c</b>) AFM images and (<b>d</b>) microstrain analysis for the OIHP films on PhNa−1T and PhNa−1T/OABr (AFM images were taken with dimensions of 4 μm × 4 μm).</p>
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<p>(<b>a</b>) UPS spectra for PhNa−1T and PhNa−1T/OABr films. (<b>b</b>) Schematic diagram for energy level alignments occurred for PhNa−1T and PhNa−1T/OABr.</p>
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18 pages, 1206 KiB  
Review
Recent Advancements in Chitosan-Based Biomaterials for Wound Healing
by Jahnavi Shah, Dhruv Patel, Dnyaneshwari Rananavare, Dev Hudson, Maxwell Tran, Rene Schloss, Noshir Langrana, Francois Berthiaume and Suneel Kumar
J. Funct. Biomater. 2025, 16(2), 45; https://doi.org/10.3390/jfb16020045 - 30 Jan 2025
Viewed by 1234
Abstract
Chitosan is a positively charged natural polymer with several properties conducive to wound-healing applications, such as biodegradability, structural integrity, hydrophilicity, adhesiveness to tissue, and bacteriostatic potential. Along with other mechanical properties, some of the properties discussed in this review are antibacterial properties, mucoadhesive [...] Read more.
Chitosan is a positively charged natural polymer with several properties conducive to wound-healing applications, such as biodegradability, structural integrity, hydrophilicity, adhesiveness to tissue, and bacteriostatic potential. Along with other mechanical properties, some of the properties discussed in this review are antibacterial properties, mucoadhesive properties, biocompatibility, high fluid absorption capacity, and anti-inflammatory response. Chitosan forms stable complexes with oppositely charged polymers, arising from electrostatic interactions between (+) amino groups of chitosan and (−) groups of other polymers. These polyelectrolyte complexes (PECs) can be manufactured using various materials and methods, which brings a diversity of formulations and properties that can be optimized for specific wound healing as well as other applications. For example, chitosan-based PEC can be made into dressings/films, hydrogels, and membranes. There are various pros and cons associated with manufacturing the dressings; for instance, a layer-by-layer casting technique can optimize the nanoparticle release and affect the mechanical strength due to the formation of a heterostructure. Furthermore, chitosan’s molecular weight and degree of deacetylation, as well as the nature of the negatively charged biomaterial with which it is cross-linked, are major factors that govern the mechanical properties and biodegradation kinetics of the PEC dressing. The use of chitosan in wound care products is forecasted to drive the growth of the global chitosan market, which is expected to increase by approximately 14.3% within the next decade. This growth is driven by products such as chitoderm-containing ointments, which provide scaffolding for skin cell regeneration. Despite significant advancements, there remains a critical gap in translating chitosan-based biomaterials from research to clinical applications. Full article
(This article belongs to the Special Issue Functional Biomaterials for Skin Wound Healing)
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Figure 1
<p>The figure depicts the different factors that affect the antibacterial properties of chitosan. Created with <a href="http://BioRender.com" target="_blank">BioRender.com</a>. Accessed on 25 November 2024.</p>
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<p>Electrostatic and hydrogen bonding interactions between chitosan and other polymers. Red color circles represent amino group (+) of chitosan and blue color circles represent different negatively charged groups. Created with <a href="http://BioRender.com" target="_blank">BioRender.com</a>. Accessed on 9 January 2025.</p>
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17 pages, 2080 KiB  
Article
Multi-Responsive Amphiphilic Hyperbranched Poly[(2-dimethyl aminoethyl methacrylate)-co-(benzyl methacrylate)]copolymers: Self-Assembly and Curcumin Encapsulation in Aqueous Media
by Foteini Ginosati, Dimitrios Vagenas, Angelica Maria Gerardos and Stergios Pispas
Materials 2025, 18(3), 513; https://doi.org/10.3390/ma18030513 - 23 Jan 2025
Viewed by 521
Abstract
In this study, we report the synthesis of amphiphilic hyperbranched poly[(2-dimethylaminoethyl methacrylate)-co-(benzyl methacrylate)] statistical copolymers with two different stoichiometric compositions using the reversible addition–fragmentation chain transfer polymerization (RAFT) technique. The selection of monomers was made to incorporate a pH and thermoresponsive polyelectrolyte (DMAEMA) [...] Read more.
In this study, we report the synthesis of amphiphilic hyperbranched poly[(2-dimethylaminoethyl methacrylate)-co-(benzyl methacrylate)] statistical copolymers with two different stoichiometric compositions using the reversible addition–fragmentation chain transfer polymerization (RAFT) technique. The selection of monomers was made to incorporate a pH and thermoresponsive polyelectrolyte (DMAEMA) component and a hydrophobic component (BzMA) to achieve amphiphilicity and study the effects of architecture and environmental factors on the behavior of the novel branched copolymers. Molecular characterization was performed through size exclusion chromatography (SEC) and spectroscopic characterization techniques (1H-NMR and FT-IR). The self-assembly behavior of the hyperbranched copolymers in aqueous media, in response to variations in pH, temperature, and ionic strength, was studied using dynamic light scattering (DLS), electrophoretic light scattering (ELS), and fluorescence spectroscopy (FS). Finally, the efficacy of the two novel copolymers to encapsulate curcumin (CUR), a hydrophobic, polyphenolic drug with proven anti-inflammatory and fluorescence properties, was established. Its encapsulation was evaluated through DLS, UV–Vis, and fluorescence measurements, investigating the change of hydrodynamic radius of the produced mixed copolymer–CUR nanoparticles in each case and their fluorescence emission properties. Full article
(This article belongs to the Special Issue Applied Stimuli-Responsive Polymer Based Materials)
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Figure 1
<p><sup>1</sup>H-NMR spectra of HB1 (green) and HB2 (blue) hyperbranched copolymers (the solvent is deuterated acetone (CD<sub>3</sub>)<sub>2</sub>CO, and the letters indicate the corresponding hydrogens in the chemical structure).</p>
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<p>SEC chromatogram for HB1 and HB2 hyperbranched copolymers.</p>
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<p>Critical aggregation concentration (CAC) determination for HB1 (<b>a</b>) and HB2 (<b>b</b>) at pH 7.</p>
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<p>Size distributions from DLS for the HB1 and HB2 hyperbranched copolymer solutions at (<b>a</b>) pH 3, (<b>b</b>) pH 7, and (<b>c</b>) pH 10.</p>
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<p>Size distributions from DLS for the HB1 (<b>a</b>) and HB2 (<b>b</b>) hyperbranched copolymer solutions as a function of temperature.</p>
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<p>Ionic strength dependence plots for (<b>a</b>) HB1 and (<b>b</b>) HB2 copolymers (polymer concentration 10<sup>−3</sup> g/mL, at pH = 7 and at a temperature of 25 °C).</p>
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<p>Comparative size distributions of HB1 and HB2 copolymers with curcumin encapsulationat 10%<span class="html-italic">w</span>/<span class="html-italic">w</span> (<b>a</b>,<b>c</b>) and 20% <span class="html-italic">w</span>/<span class="html-italic">w</span> (<b>b</b>,<b>d</b>) in different media.</p>
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<p>Fluorescence of curcumin in acetone (<b>a</b>) and of HB1 aggregates at 10%<span class="html-italic">w</span>/<span class="html-italic">w</span> and 20%<span class="html-italic">w</span>/<span class="html-italic">w</span> curcumin encapsulation (<b>b</b>) and HB2 ones at 10%<span class="html-italic">w</span>/<span class="html-italic">w</span> and 20%<span class="html-italic">w/w</span> curcumin encapsulation (<b>c</b>).</p>
Full article ">Scheme 1
<p>Reaction scheme of the synthesis of P(DMAEMA-co-BzMA) hyperbranched copolymers.</p>
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